Effect of Acid-treatment of Graphitized Carbon Supports on Performance of Fuel Cell Catalysts†

doi:10.7503/cjcu20160426

Abstract

Abstract:

The graphitized carbon black(GCB) was obtained by a high temperature(1700 ℃) treatment of the XC-72 commercial carbon black(XC-72 CB). The functional groups of GCB were modified by acid treatment. Transmission electron microscopy(TEM), X-ray diffraction, Raman spectrum and infrared spectroscopy displayed the GCB with acid treatment had a higher degree of graphitization. Oxygen-containing functional groups were introduced into the GCB surface and the ordered structure of the GCB was maintained at the same time. Nitrogen adsorption and desorption experiment showed the GCB had smaller specific surface area and less micropore compared to XC-72 CB. Thermogravimetric analysis showed that GCB had the better heat stability. Cyclic voltammetry and linear sweep voltammetry test showed that the electrochemical specific activity area(ECSA)(75.25 m²/g) and the mass activity(MA)(0.093 A/mg) of conc. H₂SO₄ and conc. HNO₃ treated GCB(abbreviated as OGCB) were higher than those of the commercial one. TEM showed the Pt/OGCB had an average particle diameter of 2.28 nm, smaller than the commercial one. After durability test of 5000 cycles, the ECSA and MA of Pt/OGCB decreased by 17.3% and 29.5%, respectively, smaller than those of Pt/C(JM)(25.1% and 42.5%). Both activity and durability performance of Pt/OGCB catalyst were better than those of commercial Pt/C(JM) catalyst in oxygen reduction reaction. In addition, in single cell test, the durability of Pt/OGCB catalyst was also better than that of the commercial catalyst. The results show that OGCB has a promising application prospect in the field of proton exchange membrane fuel cell(PEMFC) catalyst support.

Key words: Proton exchange membrane fuel cell, Graphitized carbon black, Acid treatment, Durability

CLC Number:

O646

TrendMD:

YAN Haixu, YANG Meini, ZENG Hao, PU Hongting, LIN Rui. Effect of Acid-treatment of Graphitized Carbon Supports on Performance of Fuel Cell Catalysts^†[J]. Chem. J. Chinese Universities, 2016, 37(12): 2236.

Figures/Tables 17

Fig.1 TEM image(A) and SAED pattern(B) of GCB

Fig.2 XRD patterns of XC-72 CB(a) and GCB(b)

Fig.3 Raman spectra of XC-72 CB(a) and GCB(b)

Table 1 Raman spectroscopy data of XC-72 CB before and after 1700 ℃ treatment

Sample	Half-peak width/cm^-1				I_D/I_G	I_2D/I_G
Sample	D	G		2D
XC-72 CB	260.3	84.1	898.9		3.72	0.85
GCB	45.7	58.3	48.6		0.64	1.39

Fig.4 TG(A) and DSC(B) curves of XC-72 CB(a) and GCB(b)

Fig.5 IR spectra of GCB before and after pretreatmenta. GCB; b. HNO3-GCB; c. H2SO4-GCB; d. OGCB.

Fig.6 Raman spectra of GCB before and after pretreatmenta. GCB; b. HNO3-GCB; c. H2SO4-GCB; d. OGCB.

Fig.7 TEM images of different catalysts(A) Pt/GCB; (B) Pt/HNO3-GCB; (C) Pt/H2SO4-GCB; (D) Pt/OGCB.

Fig.8 Particle size distribution of different catalysts(A) Pt/GCB; (B) Pt/HNO3-GCB; (C) Pt/H2SO4-GCB; (D) Pt/OGCB.

Fig.9 Full scan XPS spectra of the four catalysts(A), C1s XPS spectra of Pt/OGCB catalyst(B) and Pt4f XPS spectra of Pt/GCB(C), Pt/HNO3-GCB(D), Pt/H2SO4-GCB(E) and Pt/OGCB(F) catalyst(A) a. Pt/GCB; b. Pt/HNO3-GCB; c. Pt/H2SO4-GCB; d. Pt/OGCB.

Fig.10 CV curves of catalysts Pt/GCB(a), Pt/HNO3-GCB(b), Pt/H2SO4-GCB(c) and Pt/OGCB(d)

Fig.11 LSV curves of catalysts Pt/GCB(a), Pt/HNO3-GCB(b), Pt/H2SO4-GCB(c) and Pt/OGCB(d)

Fig.12 TEM images of Pt/OGCB catalysts and Pt/C(JM) after 5000 cycles accelerated durability tests(A) Pt/OGCB(after 5000 cycles); (B) Pt/C(JM)(fresh); (C) Pt/C(JM)(after 5000 cycles).

Fig.13 Prticle size distribution of Pt/OGCB catalysts and Pt/C(JM) after 5000 cycles accelerated durability tests(A) Pt/OGCB(after 5000 cycles); (B) Pt/C(JM)(fresh); (C) Pt/C(JM)(after 5000 cycles).

Fig.14 CV curves of catalysts befor(a) and after(b) 5000 cycles accelerated durability tests(A) Pt/OGCB; (B) Pt/C(JM).

Fig.15 LSV curves of catalysts before(a) and after(b) 5000 cycles accelerated durability tests(A) Pt/OGCB; (B) Pt/C(JM).

Fig.16 Single-cell performance of MEAPt/C(JM)(A) and MEAPt/OGCB(B)

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